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Insights into the effect of substrate adsorption behavior over hemelike Fe_(1)/AC single-atom catalyst

Nano Research 2022年第7期15卷 5970-5976页

作者： Jianglin Duan Yanan Zhou Yujing Ren Dan Feng Jinlong Shang Huibin Ge Jie Gao Jinlong Yang Yong Qin Interdisciplinary Research Center of Biology&Catalysis School of Life SciencesNorthwestern Polytechnical UniversityXi’an 710072China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China Analytical&Testing Center Northwestern Polytechnical UniversityXi’an 710072China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China

Unraveling the substrate adsorption structure–performance relationship is pivotal for heterogeneous carbon supported metal single-atom catalysts(M_(1)/C SACs).However,due to the complexity of the functional groups on carbon material surface,it is still a great ***,inspired by structure of enzymes,we used activated carbon(AC),which has adjustable surface oxygen functional groups(OFGs),supported atomically dispersed Fe-N_(4) sites as heme-like *** based on a combination of scanning transmission electron microscopy(STEM),X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),Mössbauer spectroscopy,Fourier transform infrared(FT-IR)characterizations,kinetics experiments and density functional theory(DFT)calculations,we revealed the effect of substrate adsorption behavior on AC support surface,that is,with the increase of carboxyl group in OFGs,the adsorbed 3,3',5,5'-tetramethylbenzidine(TMB)molecular increased,and consequently the substrate enriched on AC *** carboxyl group as well as Fe-N_(4) active sites synergistically realized high-efficiency peroxidase-like activity,just like the *** work suggests that simultaneously constructing metal single-atom active sites and specific functional groups on carbon support surface may open an avenue for engineering metal-support synergistic catalysis in M_(1)/C SACs,which can further improve catalytic performance.

关键词： single-atom catalysts heme-like carboxyl group substrate adsorption behavior peroxidase-like activity

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